RESUMO

The unique properties of topological insulators such as Bi2Se3 are intriguing for their potential implementation in novel device architectures for low power and defect-tolerant logic and memory devices. Recent improvements in the synthesis of Bi2Se3 have positioned researchers to fabricate new devices to probe the limits of these materials. The fabrication of such devices, of course, requires etching of the topological insulator, in addition to other materials including gate oxides and contacts which may impact the topologically protected surface states. In this paper, we study the impact of He+ sputtering and inductively coupled plasma Cl2 and SF6 reactive etch chemistries on the physical, chemical, and electronic properties of Bi2Se3. Chemical analysis by X-ray photoelectron spectroscopy tracks changes in the surface chemistry and Fermi level, showing preferential removal of Se that results in vacancy-induced n-type doping. Chlorine-based chemistry successfully etches Bi2Se3 but with residual Se-Se bonding and interstitial Cl species remaining after the etch. The Se vacancies and residuals can be removed with postetch anneals in a Se environment, repairing Bi2Se3 nearly to the as-grown condition. Critically, in each of these cases, angle-resolved photoemission spectroscopy (ARPES) reveals that the topologically protected surface states remain even after inducing significant surface disorder and chemical changes, demonstrating that topological insulators are quite promising for defect-tolerant electronics. Changes to the ARPES intensity and momentum broadening of the surface states are discussed. Fluorine-based etching aggressively reacts with the film resulting in a relatively thick insulating film of thermodynamically favored BiF3 on the surface, prohibiting the use of SF6-based etching in Bi2Se3 processing.

RESUMO

Semiconducting MoTe2 is one of the few two-dimensional (2D) materials with a moderate band gap, similar to silicon. However, this material remains underexplored for 2D electronics due to ambient instability and predominantly p-type Fermi level pinning at contacts. Here, we demonstrate unipolar n-type MoTe2 transistors with the highest performance to date, including high saturation current (>400 µA/µm at 80 K and >200 µA/µm at 300 K) and relatively low contact resistance (1.2 to 2 kΩ·µm from 80 to 300 K), achieved with Ag contacts and AlOx encapsulation. We also investigate other contact metals (Sc, Ti, Cr, Au, Ni, Pt), extracting their Schottky barrier heights using an analytic subthreshold model. High-resolution X-ray photoelectron spectroscopy reveals that interfacial metal-Te compounds dominate the contact resistance. Among the metals studied, Sc has the lowest work function but is the most reactive, which we counter by inserting monolayer hexagonal boron nitride between MoTe2 and Sc. These metal-insulator-semiconductor (MIS) contacts partly depin the metal Fermi level and lead to the smallest Schottky barrier for electron injection. Overall, this work improves our understanding of n-type contacts to 2D materials, an important advance for low-power electronics.

RESUMO

The interconnect half-pitch size will reach ≈20 nm in the coming sub-5 nm technology node. Meanwhile, the TaN/Ta (barrier/liner) bilayer stack has to be >4 nm to ensure acceptable liner and diffusion barrier properties. Since TaN/Ta occupy a significant portion of the interconnect cross-section and they are much more resistive than Cu, the effective conductance of an ultrascaled interconnect will be compromised by the thick bilayer. Therefore, 2D layered materials have been explored as diffusion barrier alternatives. However, many of the proposed 2D barriers are prepared at too high temperatures to be compatible with the back-end-of-line (BEOL) technology. In addition, as important as the diffusion barrier properties, the liner properties of 2D materials must be evaluated, which has not yet been pursued. Here, a 2D layered tantalum sulfide (TaSx ) with ≈1.5 nm thickness is developed to replace the conventional TaN/Ta bilayer. The TaSx ultrathin film is industry-friendly, BEOL-compatible, and can be directly prepared on dielectrics. The results show superior barrier/liner properties of TaSx compared to the TaN/Ta bilayer. This single-stack material, serving as both a liner and a barrier, will enable continued scaling of interconnects beyond 5 nm node.

RESUMO

We report an excellent growth behavior of a high-κ dielectric on ReS2, a two-dimensional (2D) transition metal dichalcogenide (TMD). The atomic layer deposition (ALD) of an Al2O3 thin film on the UV-Ozone pretreated surface of ReS2 yields a pinhole free and conformal growth. In-situ half-cycle X-ray photoelectron spectroscopy (XPS) was used to monitor the interfacial chemistry and ex-situ atomic force microscopy (AFM) was used to evaluate the surface morphology. A significant enhancement in the uniformity of the Al2O3 thin film was deposited via plasma-enhanced atomic layer deposition (PEALD), while pinhole free Al2O3 was achieved using a UV-Ozone pretreatment. The ReS2 substrate stays intact during all different experiments and processes without any formation of the Re oxide. This work demonstrates that a combination of the ALD process and the formation of weak Sâ»O bonds presents an effective route for a uniform and conformal high-κ dielectric for advanced devices based on 2D materials.

RESUMO

X-ray photoelectron spectroscopy (XPS) is one of the most used methods in a diverse field of materials science and engineering. The elemental core-level binding energies (BE) and core-level shifts (CLS) are determined and interpreted in the XPS. Oxidation is commonly considered to increase the BE of the core electrons of metal and semiconductor elements (i.e., positive BE shift due to O bonds), because valence electron charge density moves toward electronegative O atoms in the intuitive charge-transfer model. Here we demonstrate that this BE hypothesis is not generally valid by presenting XPS spectra and a consistent model of atomic processes occurring at HfO2/InP interface including negative In CLSs. It is shown theoretically for abrupt HfO2/InP model structures that there is no correlation between the In CLSs and the number of oxygen neighbors. However, the P CLSs can be estimated using the number of close O neighbors. First native oxide model interfaces for III-V semiconductors are introduced. The results obtained from ab initio calculations and synchrotron XPS measurements emphasize the importance of complementary analyses in various academic and industrial investigations where CLSs are at the heart of advancing knowledge.

RESUMO

Correlations between physical properties linking film quality with wet etch rate (WER), one of the leading figures of merit, in plasma-enhanced atomic layer deposition (PEALD) grown silicon nitride (SiN x) films remain largely unresearched. Achieving a low WER of a SiN x film is especially significant in its use as an etch stopper for technology beyond 7 nm node semiconductor processing. Herein, we explore the correlation between the hydrogen concentration, hydrogen bonding states, bulk film density, residual impurity concentration, and the WERs of PEALD SiN x using Fourier transform infrared spectrometry, X-ray reflectivity, and spectroscopic ellipsometry, etc. PEALD SiN x films for this study were deposited using hexachlorodisilane and hollow cathode plasma source under a range of process temperatures (270-360 °C) and plasma gas compositions (N2/NH3 or Ar/NH3) to understand the influence of hydrogen concentration, hydrogen bonding states, bulk film density, and residual impurity concentration on the WER. Varying hydrogen concentration and differences in the hydrogen bonding states resulted in different bulk film densities and, accordingly, a variation in WER. We observe a linear relationship between hydrogen bonding concentration and WER as well as a reciprocal relationship between bulk film density and WER. Analogous to the PECVD SiN x processes, a reduction in hydrogen bonding concentration arises from either (1) thermal activation or (2) plasma excited species. However, unlike the case with silane (SiH4)-based PECVD SiN x, PEALD SiN x WERs are affected by residual impurities of Si precursors (i.e., chlorine impurity). Thus, possible wet etching mechanisms in HF in which the WER is affected by hydrogen bonding states or residual impurities are proposed. The shifts of amine basicity in SiN x due to different hydrogen bonding states and the changes in Si electrophilicity due to Cl impurity content are suggested as the main mechanisms that influence WER in the PEALD processes.

RESUMO

The transfer-free direct growth of high-performance materials and devices can enable transformative new technologies. Here, room-temperature field-effect hole mobilities as high as 707 cm2 V-1 s-1 are reported, achieved using transfer-free, low-temperature (≤120 °C) direct growth of helical tellurium (Te) nanostructure devices on SiO2 /Si. The Te nanostructures exhibit significantly higher device performance than other low-temperature grown semiconductors, and it is demonstrated that through careful control of the growth process, high-performance Te can be grown on other technologically relevant substrates including flexible plastics like polyethylene terephthalate and graphene in addition to amorphous oxides like SiO2 /Si and HfO2 . The morphology of the Te films can be tailored by the growth temperature, and different carrier scattering mechanisms are identified for films with different morphologies. The transfer-free direct growth of high-mobility Te devices can enable major technological breakthroughs, as the low-temperature growth and fabrication is compatible with the severe thermal budget constraints of emerging applications. For example, vertical integration of novel devices atop a silicon complementary metal oxide semiconductor platform (thermal budget <450 °C) has been theoretically shown to provide a 10× systems level performance improvement, while flexible and wearable electronics (thermal budget <200 °C) can revolutionize defense and medical applications.

RESUMO

Two-dimensional materials have shown great promise for implementation in next-generation devices. However, controlling the film thickness during epitaxial growth remains elusive and must be fully understood before wide scale industrial application. Currently, uncontrolled multilayer growth is frequently observed, and not only does this growth mode contradict theoretical expectations, but it also breaks the inversion symmetry of the bulk crystal. In this work, a multiscale theoretical investigation aided by experimental evidence is carried out to identify the mechanism of such an unconventional, yet widely observed multilayer growth in the epitaxy of layered materials. This work reveals the subtle mechanistic similarities between multilayer concentric growth and spiral growth. Using the combination of experimental demonstration and simulations, this work presents an extended analysis of the driving forces behind this non-ideal growth mode, and the conditions that promote the formation of these defects. Our study shows that multilayer growth can be a result of both chalcogen deficiency and chalcogen excess: the former causes metal clustering as nucleation defects, and the latter generates in-domain step edges facilitating multilayer growth. Based on this fundamental understanding, our findings provide guidelines for the narrow window of growth conditions which enables large-area, layer-by-layer growth.

RESUMO

The topologically protected surface states of three-dimensional (3D) topological insulators have the potential to be transformative for high-performance logic and memory devices by exploiting their specific properties such as spin-polarized current transport and defect tolerance due to suppressed backscattering. However, topological insulator based devices have been underwhelming to date primarily due to the presence of parasitic issues. An important example is the challenge of suppressing bulk conduction in Bi2Se3 and achieving Fermi levels ( EF) that reside in between the bulk valence and conduction bands so that the topologically protected surface states dominate the transport. The overwhelming majority of the Bi2Se3 studies in the literature report strongly n-type materials with EF in the bulk conduction band due to the presence of a high concentration of selenium vacancies. In contrast, here we report the growth of near-intrinsic Bi2Se3 with a minimal Se vacancy concentration providing a Fermi level near midgap with no extrinsic counter-doping required. We also demonstrate the crucial ability to tune EF from below midgap into the upper half of the gap near the conduction band edge by controlling the Se vacancy concentration using post-growth anneals. Additionally, we demonstrate the ability to maintain this Fermi level control following the careful, low-temperature removal of a protective Se cap, which allows samples to be transported in air for device fabrication. Thus, we provide detailed guidance for EF control that will finally enable researchers to fabricate high-performance devices that take advantage of transport through the topologically protected surface states of Bi2Se3.

RESUMO

Atomically thin transition metal dichalcogenides (TMDs) are of interest for next-generation electronics and optoelectronics. Here, we demonstrate device-ready synthetic tungsten diselenide (WSe2) via metal-organic chemical vapor deposition and provide key insights into the phenomena that control the properties of large-area, epitaxial TMDs. When epitaxy is achieved, the sapphire surface reconstructs, leading to strong 2D/3D (i.e., TMD/substrate) interactions that impact carrier transport. Furthermore, we demonstrate that substrate step edges are a major source of carrier doping and scattering. Even with 2D/3D coupling, transistors utilizing transfer-free epitaxial WSe2/sapphire exhibit ambipolar behavior with excellent on/off ratios (â¼107), high current density (1-10 µA·µm-1), and good field-effect transistor mobility (â¼30 cm2·V-1·s-1) at room temperature. This work establishes that realization of electronic-grade epitaxial TMDs must consider the impact of the TMD precursors, substrate, and the 2D/3D interface as leading factors in electronic performance.

RESUMO

Understanding the structural stability of transition-metal dichalcogenides is necessary to avoid surface/interface degradation. In this work, the structural stability of 2H-MoTe2 with thermal treatments up to 500 °C is studied using scanning tunneling microscopy and scanning transmission electron microscopy. On the exfoliated sample surface at room temperature, atomic subsurface donors originating from excess Te atoms are observed and presented as nanometer-sized, electronically-induced protrusions superimposed with the hexagonal lattice structure of MoTe2. Under a thermal treatment as low as 200 °C, the surface decomposition-induced cluster defects and Te vacancies are readily detected and increase in extent with the increasing temperature. Driven by Te vacancies and thermal energy, intense 60° inversion domain boundaries form resulting in a "wagon wheel" morphology after 400 °C annealing for 15 min. Scanning tunneling spectroscopy identified the electronic states at the domain boundaries and the domain centers. To prevent extensive Te loss at higher temperatures, where Mo6Te6 nanowire formation and substantial desorption-induced etching effects will take place simultaneously, surface and edge passivation with a monolayer graphene coverage on MoTe2 is tested. With this passivation strategy, the structural stability of MoTe2 is greatly enhanced up to 500 °C without apparent structural defects.

RESUMO

MoS2, as a model transition metal dichalcogenide, is viewed as a potential channel material in future nanoelectronic and optoelectronic devices. Minimizing the contact resistance of the metal/MoS2 junction is critical to realizing the potential of MoS2-based devices. In this work, the Schottky barrier height (SBH) and the band structure of high work function Pd metal on MoS2 have been studied by in situ X-ray photoelectron spectroscopy (XPS). The analytical spot diameter of the XPS spectrometer is about 400 µm, and the XPS signal is proportional to the detection area, so the influence of defect-mediated parallel conduction paths on the SBH does not affect the measurement. The charge redistribution by Pd on MoS2 is detected by XPS characterization, which gives insight into metal contact physics to MoS2 and suggests that interface engineering is necessary to lower the contact resistance for the future generation electronic applications.

RESUMO

The successful realization of high-performance 2D-materials-based nanoelectronics requires integration of high-quality dielectric films as a gate insulator. In this work, we explore the integration of organic and inorganic hybrid dielectrics on MoS2 and study the chemical and electrical properties of these hybrid films. Our atomic force microscopy, X-ray photoelectron spectroscopy (XPS), Raman, and photoluminescence results show that, aside from the excellent film uniformity and thickness scalability down to 2.5 nm, the molecular layer deposition of octenyltrichlorosilane (OTS) and Al2O3 hybrid films preserves the chemical and structural integrity of the MoS2 surface. The XPS band alignment analysis and electrical characterization reveal that through the inclusion of an organic layer in the dielectric film, the band gap and dielectric constant can be tuned from â¼7.00 to 6.09 eV and â¼9.0 to 4.5, respectively. Furthermore, the hybrid films show promising dielectric properties, including a high breakdown field of â¼7.8 MV/cm, a low leakage current density of â¼1 × 10-6 A/cm2 at 1 MV/cm, a small hysteresis of â¼50 mV, and a top-gate subthreshold voltage swing of â¼79 mV/dec. Our experimental findings provide a facile way of fabricating scalable hybrid gate dielectrics on transition metal dichalcogenides for 2D-material-based flexible electronics applications.

RESUMO

Controlled growth of crystalline solids is critical for device applications, and atomistic modeling methods have been developed for bulk crystalline solids. Kinetic Monte Carlo (KMC) simulation method provides detailed atomic scale processes during a solid growth over realistic time scales, but its application to the growth modeling of van der Waals (vdW) heterostructures has not yet been developed. Specifically, the growth of single-layered transition metal dichalcogenides (TMDs) is currently facing tremendous challenges, and a detailed understanding based on KMC simulations would provide critical guidance to enable controlled growth of vdW heterostructures. In this work, a KMC simulation method is developed for the growth modeling on the vdW epitaxy of TMDs. The KMC method has introduced full material parameters for TMDs in bottom-up synthesis: metal and chalcogen adsorption/desorption/diffusion on substrate and grown TMD surface, TMD stacking sequence, chalcogen/metal ratio, flake edge diffusion and vacancy diffusion. The KMC processes result in multiple kinetic behaviors associated with various growth behaviors observed in experiments. Different phenomena observed during vdW epitaxy process are analysed in terms of complex competitions among multiple kinetic processes. The KMC method is used in the investigation and prediction of growth mechanisms, which provide qualitative suggestions to guide experimental study.

RESUMO

The electronic properties of the HfO2/MoS2 interface were investigated using multifrequency capacitance-voltage (C-V) and current-voltage characterization of top-gated MoS2 metal-oxide-semiconductor field effect transistors (MOSFETs). The analysis was performed on few layer (5-10) MoS2 MOSFETs fabricated using photolithographic patterning with 13 and 8 nm HfO2 gate oxide layers formed by atomic layer deposition after in-situ UV-O3 surface functionalization. The impedance response of the HfO2/MoS2 gate stack indicates the existence of specific defects at the interface, which exhibited either a frequency-dependent distortion similar to conventional Si MOSFETs with unpassivated silicon dangling bonds or a frequency dispersion over the entire voltage range corresponding to depletion of the HfO2/MoS2 surface, consistent with interface traps distributed over a range of energy levels. The interface defects density (Dit) was extracted from the C-V responses by the high-low frequency and the multiple-frequency extraction methods, where a Dit peak value of 1.2 × 1013 cm-2 eV-1 was extracted for a device (7-layer MoS2 and 13 nm HfO2) exhibiting a behavior approximating to a single trap response. The MoS2 MOSFET with 4-layer MoS2 and 8 nm HfO2 gave Dit values ranging from 2 × 1011 to 2 × 1013 cm-2 eV-1 across the energy range corresponding to depletion near the HfO2/MoS2 interface. The gate current was below 10-7 A/cm2 across the full bias sweep for both samples indicating continuous HfO2 films resulting from the combined UV ozone and HfO2 deposition process. The results demonstrated that impedance spectroscopy applied to relatively simple top-gated transistor test structures provides an approach to investigate electrically active defects at the HfO2/MoS2 interface and should be applicable to alternative TMD materials, surface treatments, and gate oxides as an interface defect metrology tool in the development of TMD-based MOSFETs.

RESUMO

A novel phase transition, from multilayered 2H-MoTe2 to a parallel bundle of sub-nanometer-diameter metallic Mo6 Te6 nanowires (NWs) driven by catalyzer-free thermal-activation (400-500 °C) under vacuum, is demonstrated. The NWs form along the ã11-20ã 2H-MoTe2 crystallographic directions with lengths in the micrometer range. The metallic NWs can act as an efficient hole injection layer on top of 2H-MoTe2 due to favorable band-alignment. In particular, an atomically sharp MoTe2 /Mo6 Te6 interface and van der Waals gap with the 2H layers are preserved. The work highlights an alternative pathway for forming a new transition metal dichalcogenide phase and will enable future exploration of its intrinsic transportation properties.

RESUMO

Atomic-layer-deposited La2O3 films were grown on Si with different O3 pulse times and growth temperatures. The interfacial reactions and impurity behaviors were observed using in situ X-ray photoelectron spectroscopy. Longer pulse time of O3 formed the solid SiO2 interfacial barrier layer, which suppressed La-silicate formation. Meanwhile, the carboxyl compound acting as an impurity phase was replaced with LaCO3 on increasing the O3 pulse time due to further oxidation and reaction of La. Higher growth temperatures enhanced La-silicate formation by mixed diffusion of Si and La2O3, during which most of the La2O3 phase was consumed at 400 °C. C and N impurities decreased with increasing growth temperature and completely disappear at 400 °C.

RESUMO

Atomic structures and electronic properties of MoS2/HfO2 defective interfaces are investigated extensively for future field-effect transistor device applications. To mimic the atomic layer deposition growth under ambient conditions, the impact of interfacial oxygen concentration on the MoS2/HfO2 interface electronic structure is examined. Then, the effect on band offsets (BOs) and the thermodynamic stability of those interfaces is investigated and compared with available relevant experimental data. Our results show that the BOs can be modified up to 2 eV by tuning the oxygen content through, for example, the relative partial pressure. Interfaces with hydrogen impurities as well as various structural disorders were also considered, leading to different behaviors, such as n-type doping, or introducing defect states close to the Fermi level because of the formation of hydroxyl groups. Then, our results indicate that for a well-prepared interface the electronic device performance should be better than that of other interfaces, such as III-V/high-κ, because of the absence of interface defect states. However, any unpassivated defects, if present during oxide growth, strongly affect the subsequent electronic properties of the interface. The unique electronic properties of monolayer-to-few-layered transition-metal dichalcogenides and dielectric interfaces are described in detail for the first time, showing the promising interfacial characteristics for future transistor technology.

RESUMO

In an electronic device based on two dimensional (2D) transitional metal dichalcogenides (TMDs), finding a low resistance metal contact is critical in order to achieve the desired performance. However, due to the unusual Fermi level pinning in metal/2D TMD interface, the performance is limited. Here, we investigate the electronic properties of TMDs and transition metal oxide (TMO) interfaces (MoS2/MoO3) using density functional theory (DFT). Our results demonstrate that, due to the large work function of MoO3 and the relative band alignment with MoS2, together with small energy gap, the MoS2/MoO3 interface is a good candidate for a tunnel field effect (TFET)-type device. Moreover, if the interface is not stoichiometric because of the presence of oxygen vacancies in MoO3, the heterostructure is more suitable for p-type (hole) contacts, exhibiting an Ohmic electrical behavior as experimentally demonstrated for different TMO/TMD interfaces. Our results reveal that the defect state induced by an oxygen vacancy in the MoO3 aligns with the valance band of MoS2, showing an insignificant impact on the band gap of the TMD. This result highlights the role of oxygen vacancies in oxides on facilitating appropriate contacts at the MoS2 and MoOx (x < 3) interface, which consistently explains the available experimental observations.

RESUMO

Layered semiconductor compounds represent alternative electronic materials beyond graphene. WSe2 is one of the two-dimensional materials with wide potential in opto- and nanoelectronics and is often used to construct novel three-dimensional architectures with new functionalities. Here, we report the topography and the electronic property of the WSe2 characterized by means of scanning tunneling microscopy and spectroscopy (STM and STS), X-ray photoelectron spectroscopy (XPS), and inductively coupled plasma mass spectrometry. The STM images reveal the presence of atomic-size imperfections and a variation in the electronic structure caused by the presence of defects and impurities below the detection limit of XPS. Both STS and photoemission reveal a spatial variation in the Fermi level position. The analysis of the core levels indicates the presence of different doping levels. The presence of a large concentration of defects and impurities has a strong impact on the electronic properties of the WSe2 surface. Our findings demonstrate that the growth of controllable and high quality two-dimensional materials at nanometer scale is one of the most challenging tasks that requires further attention.

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(instance:"regional") AND ( year_cluster:("2002") AND pais_afiliacao:("^iUnited States^eEstados"))(instance:"regional") AND ( year_cluster:("2002") AND pais_afiliacao:("^iUnited States^eEstados"))(instance:"regional") AND ( year_cluster:("2002") AND pais_afiliacao:("^iUnited States^eEstados"))(instance:"regional") AND ( year_cluster:("2002") AND pais_afiliacao:("^iUnited States^eEstados"))